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通过聚多巴胺和 Ag 纳米颗粒增强的短链氯化石蜡的光催化矿化作用的深入了解。

Insight into the photocatalytic mineralization of short chain chlorinated paraffins boosted by polydopamine and Ag nanoparticles.

机构信息

Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Sciences and Technology, Dalian University of Technology, Dalian 116024, PR China.

School of Petroleum and Chemical Engineering, Dalian University of Technology, Panjin Campus, Panjin 124221, PR China.

出版信息

J Hazard Mater. 2018 Oct 5;359:186-193. doi: 10.1016/j.jhazmat.2018.07.066. Epub 2018 Jul 17.

DOI:10.1016/j.jhazmat.2018.07.066
PMID:30032075
Abstract

Short chain chlorinated paraffins (SCCPs) have attracted increasing attention recently due to their widespread occurrence and persistence in the environment, long-distance transport, and bioaccumulation and toxicity. For the sake of photocatalytic elimination of SCCPs, a kind of polydopamine (PDA) based photocatalyst, echinus-like FeO@PDA-Ag hybrids have been synthesized via coating FeO with PDA by self-polymerization of dopamine and further loading silver nanoparticles by in situ reduction onto the surface of PDA shell. The photogenerated charges of FeO@PDA-Ag hybrids exhibit long lifetime from transient photovoltage signal, which is of benefit to participate in various subsequent reaction processes before their recombination. Benefiting from the coating of PDA shell and the deposition of Ag nanoparticles, FeO@PDA-Ag hybrids exhibit enhanced photocatalytic activity for the removel of SCCPs as investigated by the in situ Fourier transform infrared spectroscopy, 2.9 times as high as that of FeO, due to the reactive OH radicals. The density functional theory simulation demonstrates the key mechanism of the formation of conjugate bond in the dechlorination process as well as the final product of HCl. The simulation indicates that there are no regularities for the H-abstraction but the dechlorination usually occurs in the adjacent Cl atoms next to the C with H-abstraction.

摘要

短链氯化石蜡 (SCCPs) 由于其在环境中的广泛存在和持久性、远距离迁移、生物积累和毒性而受到越来越多的关注。为了光催化消除 SCCPs,通过多巴胺的自聚合在 FeO 表面包覆一层聚多巴胺 (PDA) ,然后通过原位还原将银纳米粒子负载到 PDA 壳上,合成了一种基于聚多巴胺 (PDA) 的光催化剂,海胆状 FeO@PDA-Ag 杂化物。从瞬态光电压信号可以看出,FeO@PDA-Ag 杂化物的光生电荷具有长寿命,这有利于在它们重新组合之前参与各种后续反应过程。得益于 PDA 壳的包覆和 Ag 纳米粒子的沉积,FeO@PDA-Ag 杂化物在原位傅里叶变换红外光谱研究中表现出增强的光催化活性,可去除 SCCPs,活性是 FeO 的 2.9 倍,这归因于活性 OH 自由基。密度泛函理论模拟表明了脱氯过程中形成共轭键以及最终产物 HCl 的关键机制。模拟表明,H 提取没有规律,但脱氯通常发生在 H 提取的 C 相邻的氯原子上。

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